4.8 Article

Porous PdWM (M = Nb, Mo and Ta) Trimetallene for High C1 Selectivity in Alkaline Ethanol Oxidation Reaction


Volume 9, Issue 5, Pages -


DOI: 10.1002/advs.202103722


ethanol oxidation reaction; high C1 selectivity; high valence metal; metallene; Pd


  1. National Natural Science Foundation of China [22002083, 51772162, 22001143, 52072197]
  2. Youth Innovation and Technology Foundation of Shandong Higher Education Institutions, China [2019KJC004]
  3. Outstanding Youth Foundation of Shandong Province, China [ZR2019JQ14]
  4. Taishan Scholar Young Talent Program [tsqn201909114, tsqn201909123]
  5. Natural Science Foundation of Shandong Province [ZR2020YQ34]
  6. Major Scientific and Technological Innovation Project [2019JZZY020405]
  7. Major Basic Research Program of Natural Science Foundation of Shandong Province [ZR2020ZD09]

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A novel trimetallic material PdWM was synthesized, with Pd50W27Nb23/C showing superior performance in EOR compared to commercial Pt/C and Pd/C. W and Nb enhanced adsorption and oxidation reactions, increasing C1 selectivity.
Direct ethanol fuel cells are among the most efficient and environmentally friendly energy-conversion devices and have been widely focused. The ethanol oxidation reaction (EOR) is a multielectron process with slow kinetics. The large amount of by-product generated by incomplete oxidation greatly reduces the efficiency of energy conversion through the EOR. In this study, a novel type of trimetallene called porous PdWM (M = Nb, Mo and Ta) is synthesized by a facile method. The mass activity (15.6 A mg(Pd)(-1)) and C1 selectivity (55.5%) of Pd50W27Nb23/C trimetallene, obtained after optimizing the compositions and proportions of porous PdWM, outperform those of commercial Pt/C (1.3 A mg(Pt)(-1), 5.9%), Pd/C (5.0 A mg(Pd)(-1), 7.2%), and Pd97W3/C bimetallene (9.5 A mg(Pd)(-1), 14.1%). The mechanism by which Pd50W27Nb23/C enhances the EOR performance is evaluated by in situ Fourier transform infrared spectroscopy and density functional theory calculations. It is found that W and Nb enhance the adsorption of CH3CH2OH and oxophilic high-valence Nb accelerates the subsequent oxidation of CO and -CHx species. Moreover, Nb promotes the cleavage of C-C bonds and increases the C1 selectivity. Pd60W28Mo12/C and Pd64W27Ta9/C trimetallene synthesized by the same method also exhibit excellent EOR performance.


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